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ROCHESTER, N.Y. | What should a photographer shoot when he’s entrusted with the very last roll of Kodachrome?

Steve McCurry took aim at the Brooklyn Bridge, Grand Central Terminal and a few human icons, too. Paul Simon, the crooner synonymous with the fabled film’s richly saturated colors, shied away. But Robert De Niro stood in for the world of filmmaking.

Then Mr. McCurry headed from his base in New York City to southern Asia, where in 1984 he shot a famous portrait of a green-eyed Afghan refugee girl that made the cover of National Geographic. In India, he snapped a tribe whose nomadic way of life is disappearing — just as Kodachrome is.

The world’s first commercially successful color film, extolled since the Great Depression for its sharpness, archival durability and vibrant yet realistic hues, “makes you think,” as Mr. Simon sings, “all the world’s a sunny day.”

Kodachrome enjoyed its mass-market heyday in the 1960s and ‘70s before being eclipsed by video and easy-to-process color negative films, the kind that prints are made from. It garnered its share of spectacular images, none more iconic than Abraham Zapruder’s reel of President Kennedy’s assassination in 1963.

But Mama Time is taking Kodachrome away, and Mr. McCurry feels the tug of nostalgia even as he loads Eastman Kodak Co.’s last manufactured roll into his Nikon F6, just as he’s done “so many tens of thousands of times.”

From that moment on, “there’s a certain amount of observation and walking around — exploring, hunting, moving,” Mr. McCurry said of his craft. “It’s not all about taking pictures. It’s about appreciating this world we live in for such a brief amount of time.

“I thought, what better way to kind of honor the memory of the film than to try and photograph iconic places and people? It’s in [my] DNA to want to tell stories where the action is, that shed light on the human condition.”

Betting its future on digital photography, Kodak discontinued the slide and motion-picture film with a production run last August in which a master sheet nearly a mile long was cut up into more than 20,000 rolls.

Mr. McCurry requested the final 36-exposure strip. After nine months of planning, he embarked in June on a six-week odyssey. Trailing him was a TV crew from National Geographic Channel, which plans to broadcast a one-hour documentary early next year.

National Geographic magazine is considering doing a spread on Mr. McCurry’s trip that would include a handful of images. All the originals are destined for air-conditioned safekeeping at the George Eastman House film and photography museum in Rochester.

Mr. McCurry relied on a digital camera to help evaluate composition, perspective and light, but choosing the moment to press the shutter was pressure-packed. Even seasoned photographers have a hard time knowing when “you’re going to get that one emotional component to the picture,” he said.